Solid-State Nuclear Magnetic Resonance of Triple-Cation Mixed-Halide Perovskites

Mixed-cation lead mixed-halide perovskites are the best candidates for perovskite-based photovoltaics, thanks to their higher efficiency and stability compared to the single-cation single-halide parent compounds. TripleMix (Cs(0.05)MA(0.14)FA(0.81)PbI(2.55)Br(0.45) with FA = formamidinium and MA = methylammonium) is one of the most efficient and stable mixed perovskites for single-junction solar cells. The microscopic reasons why triplecation perovskites perform so well are still under debate. In this work, we investigated the structure and dynamics of TripleMix by exploiting multinuclear solid-state nuclear magnetic resonance (SSNMR), which can provide this information at a level of detail not accessible by other techniques. Cs-133, C-13, H-1, and Pb-207 SSNMR spectra confirmed the inclusion of all ions in the perovskite, without phase segregation. Complementary measurements showed a peculiar longitudinal relaxation behavior for the H-1 and Pb-207 nuclei in TripleMix with respect to single-cation single-halide perovskites, suggesting slower dynamics of both organic cations and halide anions, possibly related to the high photovoltaic performances.

Automated summary

Mixed-cation lead mixed-halide perovskites, especially TripleMix, show higher efficiency and stability in perovskite-based photovoltaics. The structure and dynamics of TripleMix were investigated using multinuclear solid-state nuclear magnetic resonance (SSNMR), revealing slower dynamics of both organic cations and halide anions, which may contribute to its high photovoltaic performances.